JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Jia Zhao,Heng Zhang,Yang Shi,Mengfan Luo,Hongyu Zhou,Zhenjun Xie,Ye Du,Peng Zhou,Chuanshu He,Gang Yao,Bo Lai
Ferrate (Fe(VI)) has aroused great research interest in recent years due to its environmental benignancy and lower potential in disinfection by-product generation. However, the inevitable self-decomposition and lower reactivity under alkaline conditions severely restrict the utilization and decontamination efficiency of Fe(VI). Here, we discovered that Ru(III), a representative transition metal, could effectively activate Fe(VI) to degrade organic micropollutants, and its performance on Fe(VI) activation exceeded that of previously reported metal activators. The high-valent metal species (i.e., Fe(IV)/Fe(V) and high-valent Ru species) made a major contribution to SMX removal by Fe(VI)−Ru(III). Density functional theory calculations indicated the function of Ru(III) as a two-electron reductant, leading to the production of Ru(V) and Fe(IV) as the predominant active species. The characterization analyses proved that Ru species was deposited on ferric (hydr)oxides as Ru(III), indicating the possibility of Ru(III) as an electron shuttle with the rapid valence circulation between Ru(V) and Ru(III). This study not only develops an efficient way to activate Fe(VI) but also offers a thorough understanding of Fe(VI) activation induced by transition metals.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2016
·
IF 3.652
Yalun Hu,Isaac Nartey Oduro,Yong Huang,Yunming Fang
The structural characteristics and pyrolysis behaviors of two holocelluloses obtained from lignin-first biorefinery with Ru/C or Raney Ni as catalysts were studied in this paper. The infrared spectra of the remaining solid from the lignin-first biorefinery show that both lignin and a portion of hemicellulose were decomposed. Compared with Ru/C, Raney Ni was more effective for delignification and gave a holocellulose with higher degree of crystallinity, based on both the ratio of infrared bands (1372 cm −1 /2900 cm −1 ) and XRD analysis. The pyrolyses of holocelluloses were performed in fixed-bed and free-falling reactors, and the resulting char yields from both reactors were significantly higher than those of the parent biomass and commercial cellulose. This resulted from the cleavage of cellulose chain during the lignin-first biorefinery. Raney Ni related biorefinery cleaved cellulose chain to a higher degree.
研究领域:
生物化学
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能源科学
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材料科学
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Journal of Materials Chemistry A
·
2024
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IF 10.7
Zonglin Liu,Honglei Zhang,Dongyue Liu,Yujie Feng,Dechang Jia,Caicai Li,Qingfeng Sun,Yu Zhou,Zhenhui Kang,Baoqiang Li
The in-depth understanding of electrocatalysts is the key issue in the fields of clean energy and the chemical industry. Although various carbon-loaded active metal particle catalysts for the electrocatalytic hydrogen evolution reaction (HER) have been developed, the interaction between active metals and the substrate is still unclear. Herein, ruthenium (Ru) nanoparticles loaded on N-doped carbon dots (Ru/NCDs) were constructed to discover the critical roles of the carbon substrate as well as its interaction with Ru. Notably, we show the two critical functions of NCDs in a carbon-confined Ru system. First, the ultra-small Ru nanoparticles increase the hydrogen spillover channels. Second, the carbon substrate shows a Ru-like hydrogen adsorption capacity, supplying sufficient H sources for hydrogen spillover. Thus, the hydrogen spillover is enhanced and the HER process is accelerated. The Ru/NCDs catalyst shows superior HER activity and durability in both acidic and alkaline solutions. This work clarifies the critical role of carbon substrates in carbon-loaded catalysts.
研究领域:
电化学
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催化
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清洁能源
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材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yu Wang,Yijun Jiang,Yangyang Yuan,Li Xu,Wanting Sun,Si Wu,Qingmiao Wang,Ning Hu,Li Wang
In this study, Ni was severed as a promoter and impregnated on hydroxyapatite (HAP) to prepare a Ni-doped HAP support, and then Ru was highly dispersed onto the Ni-HAP through urea precipitation method. The synergistic effects between Ru and Ni caused a reduction in the particle size of Ru nanoparticles and an increased Ru 4+ /Ru 0 ratios, which was primarily attributed to the strong interaction between the active components and functional groups of OH - and PO 4 3- . Meanwhile, Ru/Ni-HAP possessed the highest amount of medium-strength acid sites and relatively low reduction temperatures, indicating the critical balance between acidity and redox capability. Ru/Ni-HAP exhibited superior activity with complete conversion of toluene at 280 °C and DCM at 400 °C, respectively, and such high activity can be maintained throughout the stability tests. Besides, optimal catalytic performance was observed under 600 ppm concentrations of toluene and DCM with a space velocity of 40,000 ml(g·h) −1 . These findings can provide valuable insights for the development of chlorine-resistant catalysts with promising application prospects.
研究领域:
环境科学
·
催化化学
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Lin Li,Chao Feng,Haimei Xu,Ping He,Qisong Yi,Junxiang Jiang,Lu Lin,Jin Hou,Yuanshuai Liu
The catalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is an important reaction in the sustainable production of polymers from biomass resources. To advance the environmental sustainability of this process, it is crucial to develop a catalytic system that circumvents the need for liquid alkaline media, which have been conventionally employed in HMF-to-FDCA conversion. Herein, we developed an efficient catalytic system comprising Ru nanoparticles supported on Na-type zeolite Y (Ru/Na-Y) for the base-free oxidation of HMF to FDCA. Reducing the particle size of Ru significantly enhances the activity of the Ru/Na-Y catalysts. Specifically, the optimized Ru/Na-Y-300N-200H, featuring Ru nanoparticles with an average size of ∼2.5 nm, afforded nearly 100 % HMF conversion and ∼ 85 % FDCA yield under base-free aqueous-phase conditions at 100 °C and 5 MPa air pressure. Kinetic studies further evidenced that Ru/Na-Y-300N-200H could effectively catalyze the sequential oxidation of both alcohol and aldehyde groups during the HMF-to-FDCA conversion. Comprehensive characterizations and DFT calculations elucidated the enhanced interaction between Ru centers and Na sites in the Ru/Na-Y-300N-200H due to the smallest Ru particle size. The unique Ru-Na synergistic effect was thus realized, which could facilitate the activation of O 2 and the generation of O 2 •– radicals as active oxygen species, while simultaneously boosting the rate-determining step of 5-formyl-2-furancarboxylic acid (FFCA) oxidation to FDCA, resulting in a high FDCA yield. These findings unveil promising prospects for developing advanced metal-zeolite bifunctional catalysts, which could facilitate the base-free oxidation of biomass-derived HMF into FDCA.
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PHYSICA B-CONDENSED MATTER
·
2024
·
IF 2.8
Chengxiang Lv,Xiaomeng Cheng,Jiahui Sui,Kunni Jia,Xin Dong,Mingcui Ding,Bingying Pan
We report the synthesis and superconductivity of a new Ru-based alloy Ru 3 Sb 1.75 Sn 5.25 . The single crystal and polycrystal samples were synthesized by the Sn-flux method and solid state reaction , respectively. The Ru 3 Sb 1.75 Sn 5.25 crystals were characterized by powder X-ray diffraction, electrical resistivity, magnetic susceptibility , and specific heat measurements. We find Ru 3 Sb 1.75 Sn 5.25 crystallize in the Ir 3 Ge 7 -type structure and exhibits superconductivity with onset transition temperature T c = 4.2 K. Density functional theory calculation on Ru 3 Sb 1.75 Sn 5.25 unveils multiple peaks of density of states around the Fermi level , which may explain the emergence of superconductivity . Our study provides an example compound to explore the fascinating interplay of superconductivity , electronic band structure and paramagnetism in Ru-based superconductors .
研究领域:
凝聚态物理
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材料科学
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超导物理
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电子结构理论
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Wenqian Shen,Qiang Fu,Chi Shing Tsang,Lok Wing Wong,Xiaodong Zheng,Jiong Zhao,Thuc Hue Ly
Strong metal-support interaction (SMSI) plays a critical role in enhancing the catalytic performance of electrocatalysts. Currently, effective approaches to enhance the SMSI effect in supported electrocatalysts still need to be developed, and a comprehensive atomic-level understanding of the underlying reaction mechanisms remains unclear. In this study, a novel facet-junction strategy is proposed to enhance the SMSI between the loaded Ru atoms and the Co 3 O 4 support. By modulating the ratio of exposed facet for (111)/(100) crystal plane in Co 3 O 4 , the hydrogen evolution reaction (HER) performance can be dramatically enhanced by 560% and can achieve a Pt-like HER activity with the overpotential of 45 mV. Detailed analysis with atomic-resolution integrated differential phase contrast (iDPC)-scanning transmission electron microscopy (STEM), atomic-resolution high angle annular dark field (HADDF)-STEM, and electron energy loss spectroscopy (EELS) further proved that with proper (111)/(100) crystal plane ratio, the intensified charge distribution near the facet-junction region would modify the electronic structure around the active sites. This work provides new insights to enhance the SMSI and will contribute to the rational design of highly efficient electrocatalysts for water splitting.
研究领域:
材料科学
·
电催化
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Zheng Shen,Rui Xu,Guangxian Wang,Haifang Wang,Deyan Xu,JingJing Liu,Guanjie Wang,Yemin Guo,Xia Sun
In this study, a signal amplification strategy was developed, which tris (2, 2′-bipyridyl) ruthenium (II) (Ru(bpy) 3 2+ ) was incorporated as a guest molecule into the preparation system of lanthanide-based metal-organic framework (MOF). This strategy relied on strong electrostatic interactions and coordination competition to influence the growth process of the MOF, resulting in the firm immobilization of Ru(bpy) 3 2+ within the MOF structure. The spatial confinement effect of the MOF effectively improved the efficiency of electron transfer in the electrochemiluminescence (ECL) reaction. The constructed ECL aptasensor using this MOF exhibited excellent performance, with limits of detection (LODs) for four organophosphorus pesticides (OPs), phorate, profenofos, isocarbophos and omethoate, as low as 0.0482 ng/mL, 0.0093 ng/mL, 0.0085 ng/mL, and 0.0893 ng/mL, respectively. This work has paved the way for a clever strategy of immobilizing Ru(bpy) 3 2+ molecules and amplifying signals, expanding the application of dual-ligand MOF, which provides valuable insights for future biosensor design.
研究领域:
分析化学
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环境科学
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MOLECULES
·
2025
·Vol. 30
·期 8
·1780
·
IF 4.6
Shiying Yang,Xin Jin,Bin Zhu,Dan Yang,Xiaoyue Wan,Yihu Dai,Chunmei Zhou,Yuguang Jin,Yanhui Yang
5-Hydroxymethylfurfural (HMF) serves as an important bridge connecting biomass resources with fossil fuels. Its downstream product, 2,5-furandicarboxylic acid (FDCA), is a renewable alternative to terephthalic acid (TPA) in the synthesis of various polymer materials. In this study, we successfully synthesized four ruthenium-based catalysts with varying valence states supported on carbon nanotubes (CNTs) and compared the performance of HMF electrooxidation. Among these, the Ru+2.9catalyst demonstrated the highest activity for the electrochemical oxidation of HMF to FDCA in the neutral medium (0.1 M K2SO4). Notably, the FDCA yield reached 90.2% under an applied potential of 0.95 V (vs. Ag/AgCl) after 24 h. Mechanistic analysis revealed that the superior specific capacitance of the Ru+2.9catalyst significantly facilitated the reaction process. This work represents a more cost-effective approach to avoid the need for excessive alkaline additives during catalyst preparation and the HMF oxidation process, and FDCA separated easily after cooling the reaction solution down.
研究领域:
能源化学
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催化化学
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生物质转化
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Jialian Ding,Bin Su
Graphical One plus one is greater than two: A remarkable electrochemiluminescence (ECL) enhancement of Ru(bpy) 3 2+ /TPrA is observed by introducing another coreactant, TEOA, with a 10.8-fold increase of ECL intensity and 1.7-fold extension of ECL layer. The enhancement was interpreted by a chemical oxidation route, in which TEOA + ⋅ acts as an enhancer to produce more TPrA + ⋅ and meanwhile allow the remote formation of TPrA + ⋅. This dual-coreactants strategy works not only in solution with freely diffusive Ru(bpy) 3 2+ but also on Ru(bpy) 3 2+ -functionalized microbeads, showing promise in ECL-based bioassay and microscopy. The electrochemiluminescence (ECL) of ruthenium(II) tris(2,2′-bipyridyl) (Ru(bpy) 3 2+ ) with tri- n -propylamine (TPrA) as the good coreactant can be unexpectedly enhanced by a weak coreactant, such as triethanolamine (TEOA). First, the intensity of ECL emitted by Ru(bpy) 3 2+ /TPrA can be remarkably amplified by 10.8-fold after adding some amount of TEOA. Moreover, the ECL layer thickness, measured by self-interference spectroscopy, is also doubled. The enhancement far exceeding the superposition of respective contribution of TPrA and TEOA was elucidated by a “chemical oxidation mechanism”, in which TEOA + ⋅ acts as a chemical enhancer to oxidize TPrA in solution and to accelerate significantly the ECL reaction kinetics. This mechanism was proved by single-photon counting experiment and finite element simulations. In addition, the dual-coreactants strategy works well not only in solution with freely diffusive Ru(bpy) 3 2+ , but also on Ru(bpy) 3 2+ -functionalized microbeads, suggesting that ethanolamines could act as cheap, easily available and low-background enhancers for ECL-based bioanalysis and microscopy.
研究领域:
分析化学
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生物分析
·
显微技术
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 35
·15169-15176
·
IF 3.288
Gang Zhang,Tong Chen,Yi Zhang,Tao Liu,Gongying Wang
Ru–carbon catalysts with different physical morphologies and chemical states of Ru were prepared by different methods and used to catalyze the hydrolytic hydrogenation of cellulose at high temperatures. The physical morphology of Ru particles and the chemical state of Ru significantly influenced the catalytic performance. The Ru nanoparticles in Ru@MC prepared by the in situ carbothermal reduction method exhibited a special chemical state due to the strong interaction with carbon. The special structure could not only prevent the growth of Ru particles but also enhance the hydrogen spillover effect and improve the hydrogenation efficiency. Among the Ru–carbon catalysts, Ru@MC showed the best catalytic performance with a 72.4% yield of sorbitol. Furthermore, the embedded structure of Ru@MC stabilized the Ru nanoparticles, and the catalyst could be reused at least 6 times.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 12
·8556-8563
·
IF 3.3
Zijian Wang,Jiaxin Zhang,Lele Yan,Bo Zhao,Lin Zheng,Haoran Guo,Yuxue Yue,Deman Han,Xianlang Chen,Rongrong Li
4-Chloroaniline (4-CAN) plays an important role in chemical and industrial production. However, it remains a challenge to avoid the hydrogenation of the C–Cl bond in the synthesis process to improve selectivity under high activity conditions. In this study, we in situ fabricated ruthenium nanoparticles (Ru NPs) containing vacancies inserted into porous carbon (Ru@C-2) as a highly efficient catalyst for the catalytic hydrogenation of 4-chloronitrobenzene (4-CNB) with remarkable conversion (99.9%), selectivity (99.9%), and stability. Experiments and theoretical calculations indicate that the appropriate Ru vacancies affect the charge distribution of the Ru@C-2 catalyst, promote the electron transfer between the Ru metal and support, and increase the active sites of the Ru metal, thus facilitating the adsorption of 4-CNB and the desorption of 4-CAN to improve the activity and stability of the catalyst. This study can provide some enlightenment for the development of new 4-CNB hydrogenation catalysts.
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